A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis

doi:10.1002/adma.202406403

IMR OpenIR

	A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis
	Liu, Wei 1; Chen, Rui 1; Sang, Zhiyuan 1; Li, Zhenxin 1; Nie, Jiahuan 1; Yin, Lichang 2; Hou, Feng 1; Liang, Ji 1
通讯作者	Sang, Zhiyuan(sangzhiyuan@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn)
	2024-07-22
发表期刊	ADVANCED MATERIALS
ISSN	0935-9648
页码	10
摘要	Designing non-noble metal single-atom catalysts (M-SACs) for two-electron oxygen reduction reaction (2e-ORR) is attractive for the hydrogen peroxide (H2O2) electrosynthesis, in which the coordination configuration of the M-SACs essentially affects the reaction activity and product selectivity. Though extensively investigated, a generalized coordination engineering strategy has not yet been proposed, which fundamentally hinders the rational design of M-SACs with optimized catalytic capabilities. Herein, a generalized coordination engineering strategy is proposed for M-SACs toward H2O2 electrosynthesis via introducing heteroatoms (e.g., oxygen or sulfur atoms) with higher or lower electronegativity than nitrogen atoms into the first sphere of metal-N4 system to tailor their electronic structure and adjust the adsorption strength for *OOH intermediates, respectively, thus optimizing their electrocatalytic capability for 2e-ORR. Specifically, the (O, N)-coordinated Co SAC (Co-N3O) and (S, N)-coordinated Ni SAC (Ni-N3S) are precisely synthesized, and both present superior 2e-ORR activity (Eonset: approximate to 0.80 V versus RHE) and selectivity (approximate to 90%) in alkaline conditions compared with conventional Co-N4 and Ni-N4 sites. The high H2O2 yield rates of 14.2 and 17.5 moL g-1 h-1 and long-term stability over 12 h are respectively achieved for Co-N3O and Ni-N3S. Such favorable 2e-ORR pathway of the catalysts is also theoretically confirmed by the kinetics simulations. During the generalized coordination engineering strategy, the representative samples Co-N3O and Ni-N3S are precisely synthesized, and both of them present excellent activity and H2O2 selectivity (approximate to 90%) compared with conventional Metal-N4 configurations. Moreover, they enable a high H2O2 production of 14.2 and 17.5 moL g-1 h-1 in the three-phrase flow cell and maintain a satisfying stability over 12 h. image
关键词	2e-ORR metal-organic frameworks single-atom catalysts
资助者	National Natural Science Foundation of China
DOI	10.1002/adma.202406403
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[22379111] ; National Natural Science Foundation of China[22179093]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001273242900001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：21[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/188382
专题	中国科学院金属研究所
通讯作者	Sang, Zhiyuan; Liang, Ji
作者单位	1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Liu, Wei,Chen, Rui,Sang, Zhiyuan,et al. A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis[J]. ADVANCED MATERIALS,2024:10.
APA	Liu, Wei.,Chen, Rui.,Sang, Zhiyuan.,Li, Zhenxin.,Nie, Jiahuan.,...&Liang, Ji.(2024).A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis.ADVANCED MATERIALS,10.
MLA	Liu, Wei,et al."A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis".ADVANCED MATERIALS (2024):10.